US7897530B2 - Glass-ceramic sealant for planar solid oxide fuel cells - Google Patents

Glass-ceramic sealant for planar solid oxide fuel cells Download PDF

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Publication number
US7897530B2
US7897530B2 US12/007,696 US769608A US7897530B2 US 7897530 B2 US7897530 B2 US 7897530B2 US 769608 A US769608 A US 769608A US 7897530 B2 US7897530 B2 US 7897530B2
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United States
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mol
sealant
glass
oxide
ceramic
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Expired - Fee Related, expires
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US12/007,696
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US20100184580A1 (en
Inventor
Chien-Kuo Liu
Tung-Yuan Yung
Kin-Fu Lin
Ruey-Yi Lee
Tzang-Sheng Lee
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Institute of Nuclear Energy Research
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Institute of Nuclear Energy Research
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Priority to US12/007,696 priority Critical patent/US7897530B2/en
Assigned to ATOMIC ENERGY COUNCIL - INSTITUTE OF NUCLEAR ENERGY RESEARCH reassignment ATOMIC ENERGY COUNCIL - INSTITUTE OF NUCLEAR ENERGY RESEARCH ASSIGNMENT OF ASSIGNORS INTEREST (SEE DOCUMENT FOR DETAILS). Assignors: LEE, RUEY-YI, LEE, TZANG-SHENG, LIN, KIU-FU, LIU, CHIEN-KUO, YUNG, TUNG-YUAN
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    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C8/00—Enamels; Glazes; Fusion seal compositions being frit compositions having non-frit additions
    • C03C8/02—Frit compositions, i.e. in a powdered or comminuted form
    • C—CHEMISTRY; METALLURGY
    • C03—GLASS; MINERAL OR SLAG WOOL
    • C03C—CHEMICAL COMPOSITION OF GLASSES, GLAZES OR VITREOUS ENAMELS; SURFACE TREATMENT OF GLASS; SURFACE TREATMENT OF FIBRES OR FILAMENTS MADE FROM GLASS, MINERALS OR SLAGS; JOINING GLASS TO GLASS OR OTHER MATERIALS
    • C03C8/00—Enamels; Glazes; Fusion seal compositions being frit compositions having non-frit additions
    • C03C8/24—Fusion seal compositions being frit compositions having non-frit additions, i.e. for use as seals between dissimilar materials, e.g. glass and metal; Glass solders
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/02—Details
    • H01M8/0271—Sealing or supporting means around electrodes, matrices or membranes
    • H01M8/028—Sealing means characterised by their material
    • H01M8/0282—Inorganic material
    • H—ELECTRICITY
    • H01—ELECTRIC ELEMENTS
    • H01M—PROCESSES OR MEANS, e.g. BATTERIES, FOR THE DIRECT CONVERSION OF CHEMICAL ENERGY INTO ELECTRICAL ENERGY
    • H01M8/00—Fuel cells; Manufacture thereof
    • H01M8/10—Fuel cells with solid electrolytes
    • H01M8/12—Fuel cells with solid electrolytes operating at high temperature, e.g. with stabilised ZrO2 electrolyte
    • H01M2008/1293—Fuel cells with solid oxide electrolytes
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02E—REDUCTION OF GREENHOUSE GAS [GHG] EMISSIONS, RELATED TO ENERGY GENERATION, TRANSMISSION OR DISTRIBUTION
    • Y02E60/00—Enabling technologies; Technologies with a potential or indirect contribution to GHG emissions mitigation
    • Y02E60/30—Hydrogen technology
    • Y02E60/50—Fuel cells

Definitions

  • the present invention relates to planar solid oxide fuel cells and, more particularly, to glass-ceramic sealant for planar solid oxide fuel cells.
  • Solid oxide fuel cells are high-temperature fuel cells of high generation efficiencies.
  • planar solid oxide fuel cells include the simplest structures, provide the highest generation efficiencies and involve the lowest working temperatures. Therefore, the planar solid oxide fuel cells are the focus of the research and development of solid oxide fuel cells.
  • a planar solid oxide fuel cell includes a PEN and an anode, a cathode, a solid electrolyte and a bi-polar inter-connector stacked on one another.
  • the anode, the cathode and the solid electrolyte together are called the “PEN.”
  • the anode, the cathode and the solid electrolyte are made of ceramics.
  • the bi-polar inter-connector is made of stainless steel.
  • the present invention is therefore intended to obviate or at least alleviate the problems encountered in prior art.
  • the primary objective of the present invention is to provide glass-ceramic sealant for planar solid oxide fuel cells.
  • the Glass-ceramic sealant for planar solid oxide fuel cells.
  • the glass-ceramic sealant includes 0 to 40 mol % of silicon oxide, 0 to 15 mol % boron oxide, 0 to 10 mol % of aluminum oxide, 0 to 40 mol % of barium oxide, 0 to 15 mol % of calcium oxide, 0 to 15 mol % of lanthanum oxide and 0 to 5 mol % of zirconium dioxide.
  • the thermal expansion coefficient of the sealant is 8 to 10 ppm/° C.
  • FIG. 1 is a flow chart of a method for making glass-ceramic sealant for planar solid oxide fuel cells according to the preferred embodiment of the present invention.
  • FIG. 2 is chart of thermal expansion coefficients vs. temperature of the glass-ceramic sealant made according to the method shown in FIG. 1 .
  • FIG. 1 there is shown a method for making glass-ceramic sealant for solid oxide fuel cells according to the preferred embodiment of the present invention.
  • a mixture is provided with 34 mol % of silicon oxide, 9.5 mol % of boron oxide, 4.5 mol % of aluminum oxide, 34 mol % of barium oxide, 12 mol % of calcium oxide, 5 mol % of lanthanum oxide and 1 mol % of zirconium dioxide.
  • the mixture is disposed in a crucible and heated in a furnace.
  • the temperature is raised to 500° C. at a temperature gradient of 5° C./min.
  • the temperature is retained at 500° C. for 1 hour. Then, the temperature is raised to 1550° C. at the same temperature gradient. The temperature is retained at 1550° C. for at least 10 hours so that liquid of molten glass is provided. The molten glass is quenched to the zoom temperature and turned into sealant for planar solid oxide fuel cells.
  • the liquid of molten glass may be quenched to the annealing point for at least 10 hours. Finally, the liquid of molten glass is slowly cooled to the zoom temperature, thus removing residual stress that would otherwise exist therein.
  • the thermal expansion coefficient of a high-chromium stainless steel bi-polar inter-connector is shown in a line 21 .
  • the thermal expansion coefficient of the high-chromium stainless steel bi-polar inter-connector is about 11.0 ppm/° C.
  • the thermal expansion coefficient of a PEN is shown in a line 22 .
  • the thermal expansion coefficient of a PEN is about 10.2 ppm/° C.
  • the thermal expansion coefficient of the sealant is shown in a line 23 .
  • the thermal expansion coefficient of the sealant is about 10 ppm/° C.
  • the transition point of the sealant is 625° C. while the softening point is 745° C.
  • the thermal expansion coefficient of the sealant is close to those of the high-chromium stainless steel bi-polar inter-connector and the PEN.
  • the sealant is used to seal the high-chromium stainless steel bi-polar inter-connector and the PEN to provide a planar solid oxide fuel cell, there will be only a small amount of thermal stress in the planar solid oxide fuel cell in operation. Hence, the sealant provides excellent air-tightness and isolation.
  • the sealant includes 0 to 40 mol % of silicon oxide, 0 to 15 mol % boron oxide, 0 to 10 mol % of aluminum oxide, 0 to 40 mol % of barium oxide, 0 to 15 mol % of calcium oxide, 0 to 15 mol % of lanthanum oxide and 0 to 5 mol % of zirconium dioxide.
  • the thermal expansion coefficient of the sealant is 8 to 10 ppm/° C.
  • the softening point of the sealant is 680° C. to 750° C.
  • the sealant can be provided between two metal layers or two ceramic layers or between a metal layer and a ceramic layer.
  • the sealant can be used for planar solid oxide fuel cells for air-tightness and sealing.

Abstract

Glass-ceramic sealant is disclosed for planar solid oxide fuel cells. The glass-ceramic sealant includes 0 to 40 mol % of silicon oxide, 0 to 15 mol % boron oxide, 0 to 10 mol % of aluminum oxide, 0 to 40 mol % of barium oxide, 0 to 15 mol % of calcium oxide, 0 to 15 mol % of lanthanum oxide and 0 to 5 mol % of zirconium dioxide. At 0° C. to 600° C., the thermal expansion coefficient of the sealant is 8 to 10 ppm/° C.

Description

BACKGROUND OF INVENTION
1. Field of Invention
The present invention relates to planar solid oxide fuel cells and, more particularly, to glass-ceramic sealant for planar solid oxide fuel cells.
2. Related Prior Art
Solid oxide fuel cells are high-temperature fuel cells of high generation efficiencies. Among the solid fuel cells, planar solid oxide fuel cells include the simplest structures, provide the highest generation efficiencies and involve the lowest working temperatures. Therefore, the planar solid oxide fuel cells are the focus of the research and development of solid oxide fuel cells.
A planar solid oxide fuel cell includes a PEN and an anode, a cathode, a solid electrolyte and a bi-polar inter-connector stacked on one another. The anode, the cathode and the solid electrolyte together are called the “PEN.” The anode, the cathode and the solid electrolyte are made of ceramics. The bi-polar inter-connector is made of stainless steel. These components of the planar solid oxide fuel cell are joined together by sealant. The thermal expansion coefficients of the sealant are very different from the thermal expansion coefficients of the components. The temperature differs from point to point in the sealant and the components. Hence, there is considerable thermal stress in the planar solid oxide fuel cell. Such thermal stress might cause the sealant to crack and the components to peel from one another. The components might be exposed and/or damaged. The generation efficiency of the planar solid oxide fuel cell might be reduced. In the worst scenario, the planar solid oxide fuel cell might be out of order.
The present invention is therefore intended to obviate or at least alleviate the problems encountered in prior art.
SUMMARY OF INVENTION
The primary objective of the present invention is to provide glass-ceramic sealant for planar solid oxide fuel cells.
To achieve the foregoing objective the Glass-ceramic sealant is disclosed for planar solid oxide fuel cells. The glass-ceramic sealant includes 0 to 40 mol % of silicon oxide, 0 to 15 mol % boron oxide, 0 to 10 mol % of aluminum oxide, 0 to 40 mol % of barium oxide, 0 to 15 mol % of calcium oxide, 0 to 15 mol % of lanthanum oxide and 0 to 5 mol % of zirconium dioxide. At 0° C. to 600° C., the thermal expansion coefficient of the sealant is 8 to 10 ppm/° C.
Other objectives, advantages and features of the present invention will become apparent from the following description referring to the attached drawings.
BRIEF DESCRIPTION OF DRAWINGS
The present invention will be described via the detailed illustration of the preferred embodiment referring to the drawings.
FIG. 1 is a flow chart of a method for making glass-ceramic sealant for planar solid oxide fuel cells according to the preferred embodiment of the present invention.
FIG. 2 is chart of thermal expansion coefficients vs. temperature of the glass-ceramic sealant made according to the method shown in FIG. 1.
 DETAILED DESCRIPTION OF PREFERRED EMBODIMENT
Referring to FIG. 1, there is shown a method for making glass-ceramic sealant for solid oxide fuel cells according to the preferred embodiment of the present invention.
At 11, a mixture is provided with 34 mol % of silicon oxide, 9.5 mol % of boron oxide, 4.5 mol % of aluminum oxide, 34 mol % of barium oxide, 12 mol % of calcium oxide, 5 mol % of lanthanum oxide and 1 mol % of zirconium dioxide.
At 12, the mixture is disposed in a crucible and heated in a furnace. The temperature is raised to 500° C. at a temperature gradient of 5° C./min.
The temperature is retained at 500° C. for 1 hour. Then, the temperature is raised to 1550° C. at the same temperature gradient. The temperature is retained at 1550° C. for at least 10 hours so that liquid of molten glass is provided. The molten glass is quenched to the zoom temperature and turned into sealant for planar solid oxide fuel cells.
Alternatively, the liquid of molten glass may be quenched to the annealing point for at least 10 hours. Finally, the liquid of molten glass is slowly cooled to the zoom temperature, thus removing residual stress that would otherwise exist therein.
Referring to FIG. 2, the thermal expansion coefficient of a high-chromium stainless steel bi-polar inter-connector is shown in a line 21. The thermal expansion coefficient of the high-chromium stainless steel bi-polar inter-connector is about 11.0 ppm/° C. The thermal expansion coefficient of a PEN is shown in a line 22. The thermal expansion coefficient of a PEN is about 10.2 ppm/° C. The thermal expansion coefficient of the sealant is shown in a line 23. The thermal expansion coefficient of the sealant is about 10 ppm/° C. The transition point of the sealant is 625° C. while the softening point is 745° C.
As discussed, the thermal expansion coefficient of the sealant is close to those of the high-chromium stainless steel bi-polar inter-connector and the PEN. When the sealant is used to seal the high-chromium stainless steel bi-polar inter-connector and the PEN to provide a planar solid oxide fuel cell, there will be only a small amount of thermal stress in the planar solid oxide fuel cell in operation. Hence, the sealant provides excellent air-tightness and isolation.
According to the present invention, the sealant includes 0 to 40 mol % of silicon oxide, 0 to 15 mol % boron oxide, 0 to 10 mol % of aluminum oxide, 0 to 40 mol % of barium oxide, 0 to 15 mol % of calcium oxide, 0 to 15 mol % of lanthanum oxide and 0 to 5 mol % of zirconium dioxide. At 0° C. to 600° C., the thermal expansion coefficient of the sealant is 8 to 10 ppm/° C. The softening point of the sealant is 680° C. to 750° C. The sealant can be provided between two metal layers or two ceramic layers or between a metal layer and a ceramic layer. The sealant can be used for planar solid oxide fuel cells for air-tightness and sealing.
The present invention has been described via the detailed illustration of the preferred embodiment. Those skilled in the art can derive variations from the preferred embodiment without departing from the scope of the present invention. Therefore, the preferred embodiment shall not limit the scope of the present invention defined in the claims.

Claims (4)

1. A glass-ceramic sealant consisting essentially of 34 mol % of silicon oxide, 9.5 mol % boron oxide, 4.5 mol % aluminum oxide, 34 mol % barium oxide, 12 mol % calcium oxide, 5 mol % lanthanum oxide, and 1 mol % zirconium dioxide.
2. The glass-ceramic sealant according to claim 1, wherein the thermal expansion coefficient of the sealant is 8 to 10 ppm/° C. at 0° C. to 600° C.
3. The glass-ceramic sealant according to claim 1, wherein the softening point of the sealant is 680° C. to 750° C.
4. The glass-ceramic sealant according to claim 1, wherein the sealant has a coefficient of thermal expansion within 1 ppm/° C. of coefficients of thermal expansion of one or both of a metal layer and a ceramic layer adjacent the glass-ceramic sealant.
US12/007,696 2008-01-14 2008-01-14 Glass-ceramic sealant for planar solid oxide fuel cells Expired - Fee Related US7897530B2 (en)

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Cited By (2)

* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2014018536A1 (en) * 2012-07-23 2014-01-30 Mo-Sci Corporation Viscous sealing glass compositions for solid oxide fuels cells
CN104531975A (en) * 2014-12-06 2015-04-22 苏州欣航微电子有限公司 Electric bicycle flywheel quenching coating apparatus

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CN102530963B (en) * 2011-10-12 2013-04-10 邱富仁 Rotary type self-resistance heating pickling kettle
JP5840937B2 (en) * 2011-11-25 2016-01-06 京セラ株式会社 Glass ceramic sintered body, reflecting member and light emitting element mounting substrate using the same, and light emitting device
US9067818B2 (en) * 2012-01-19 2015-06-30 General Electric Company Sealing glass composition and article
WO2014107631A1 (en) * 2013-01-04 2014-07-10 Lilliputian Systems, Inc. High temperature substrate attachment glass
WO2015046195A1 (en) * 2013-09-30 2015-04-02 日本山村硝子株式会社 Glass composition for sealing

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JPS63218525A (en) * 1987-03-05 1988-09-12 Nippon Electric Glass Co Ltd Glass for sealing fe-ni-co alloy
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* Cited by examiner, † Cited by third party
Publication number Priority date Publication date Assignee Title
WO2014018536A1 (en) * 2012-07-23 2014-01-30 Mo-Sci Corporation Viscous sealing glass compositions for solid oxide fuels cells
US9530991B2 (en) 2012-07-23 2016-12-27 Mo-Sci Corporation Viscous sealing glass compositions for solid oxide fuel cells
CN104531975A (en) * 2014-12-06 2015-04-22 苏州欣航微电子有限公司 Electric bicycle flywheel quenching coating apparatus

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